Metallic glasses have attracted extensive interest for outstanding properties, yet their intrinsic atomic disorder makes precise composition design highly challenging. In this work, we develop a suite of computational methods to predict the key properties of metallic glasses and to accelerate their composition development. A machine learning interatomic potential for metallic glasses is established using a dataset of 20,400 configurations from 19 representative binary and ternary systems. The model demonstrates excellent predictive performance on an independent test set, with a mean absolute error of 5.06 meV/atom for energy, 128.51 meV/A & ring; for force, and 0.17 GPa for stress. Based on this model, automated simulation workflows are further developed for density, Young's modulus, and glass transition temperature, enabling quantitative high-throughput property mapping. The calculated trends are in good agreement with the experimental results. As a representative validation case, Co-Ir-Ta-B metallic glasses are investigated. The simulations show that the decrease in Young's modulus is associated with a structurally loosened atomic packing state, and the largely preserved coordination environment supports the validity of the similarelement substitution strategy. Overall, the proposed framework provides a screening-oriented computational route for quantitative property mapping and offers atomistic structural evidence to rationalize experimentally observed property trends. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Li-rich alloys with multiphase structures have emerged as highly promising anode materials for high-energydensity Li metal batteries (LMBs). However, the variation in lithiophilicity among distinct phase domains often leads to non-uniform Li nucleation and inferior reversibility of Li deposition/dissolution. Herein, we construct a lithiophilic-equipotential Li-Cu-Mg ternary Li-rich alloy anode by synchronously doping highly lithiophilic Mg into all phases of the Li-rich Li-Cu alloy. Density functional theory (DFT) calculations revealed that the Li adsorption energies at the thermodynamically stable sites of Li-Mg and LixCu2Mg phases in the Li-CuMg ternary system are closely matched (-1.11 eV and -1.27 eV, respectively), effectively eliminating the lithiophilicity difference between the two phases. This similarity could ensure nearly identical nucleation overpotentials during Li deposition, thereby enabling the precise regulation of Li plating behavior as well as achieving homogeneous and dense Li morphology. The assembled Li-Cu-Mg@Cu symmetric cell can deliver a long cycling lifespan of over 2000 h with a stable polarization voltage of 14 mV at 1 mA cm- 2/1 mAh cm- 2. Furthermore, the full cell coupling a 35 mu m-thick Li-Cu-Mg@Cu anode with LiFePO4 (LFP) cathode (1.69 mAh cm- 2) can retain a high capacity retention of 92.9% after 600 cycles at 1 C.

The simple superposition of multiple gradient structures in three-dimensional (3D) Li anodes can, in principle, integrate the advantages of individual gradients to further regulate Li deposition. However, this "mere superposition" approach often fails to deliver satisfactory cycling stability, and no definitive guideline for achieving true gradient synergistic effects is available. Here, we propose that enhancing the all-space Li+ transport kinetics should serve as the core principle for 3D Li anode gradients designing. Through a facile thermal-compounding process, a 50 mu m-thick Li-Mg-Sn alloy film and carbon cloth (CC) sheet are tightly integrated on the stainless-steel substrate at elevated temperature, forming a lithiophilically modified carbon fiber skeleton. Simultaneously, a co-originated dual-gradient structure-comprising pore-size gradient and ion-transport-pathway gradient-is formed in situ within the skeleton. The two ion-transport pathways at the bottom offset the limited Li+ diffusion in small pores, boosting all-space Li+ transport kinetics throughout the 3D host and guiding preferential Li deposition at the electrode bottom. The symmetric cell sustains cycling stability over 5000 h with an ultralow polarization voltage of similar to 14 mV at 1 mA cm(-2)/1 mAh cm(-2) and >1200 h at 3 mA cm(-2)/3 mAh cm(-2). When paired with a LiFePO4 cathode (1.69 mAh cm(-2)), the full cell retains 80% capacity after 1300 cycles at 1 C. This dual-gradient synergistic coupling ensures rapid Li+ transport across the entire electrode, fundamentally enabling a bottom-up Li-plating, significantly extending the cycle life of the 3D Li composite anode, and providing insights for future gradient design.

All-solid-state batteries (ASSBs) require solid electrolytes with both high ionic conductivity and favorable mechanical properties to maintain intimate interfacial contact with electrode particles during cycling. Herein, we report a new silicon-based solid electrolyte, Li2SiI4O, designed through theoretical calculations and subsequently synthesized experimentally. For an ideal amorphous deep-eutectic Li2SiI4O system, theoretical calculations predict a Young's modulus below 5 GPa, suggesting excellent mechanical compliance and potential plasticity. Indeed, the experimentally synthesized Li2SiI4O exhibits a Young's modulus of 19.8 GPa, lower than that of typical sulfide solid electrolytes with Young's modulus of approximately 23 GPa. This relatively low modulus is expected to improve interfacial contact between the active electrode materials and the solid electrolyte, resembling the conformal contact commonly observed at solid–liquid interfaces. Electrochemical impedance spectroscopy measurements show that Li2SiI4O exhibits an ionic conductivity of 1.23 × 10−4 S/cm at room temperature. When employed as the solid electrolyte in ASSBs, the assembled cells deliver stable cycling performance with 80% capacity retention after 800 cycles. These results demonstrate that Li2SiI4O is a promising solid electrolyte candidate for practical ASSBs by combining favorable mechanical compliance with stable electrochemical performance.

Disordered rock-salt (DRX) cathodes offer a promising pathway for high-energy-density lithium-ion batteries using earth-abundant elements. However, the vast chemical design space and the presence of short-range ordering make systematic experimental exploration and first-principles modeling prohibitively expensive, hindering rational materials discovery. Here, we propose a data-driven design strategy via a physically informed deep learning framework based on a graph neural network (GNN) to speed up the development of DRX cathodes. It is capable of bridging the complex relationships between DRX composition and electrochemical performance using only composition-level inputs and discharge conditions, lifting the necessity of conducting complicated structural characterization or expensive multi-scale simulation. By constructing chemically meaningful elemental and ionic descriptors and employing rigorous collinearity screening, our model achieves robust predictive performance on limited datasets while improving descriptor-level physical transparency relative to embeddingbased approaches. We validate the model's capability of capturing the impact of subtle compositional variations on the electrochemical performance. Furthermore, we deploy the model to efficiently screen for optimal DRX compositions across high-dimensional chemical spaces involving different combinations of d0 and non-d0 transition-metal species. This work establishes an efficient and robust data-driven paradigm for accelerating DRX cathode discovery and provides a foundation for integrating machine learning into autonomous materials design workflows for next-generation lithium-ion batteries.

ABSTRACT The capacity utilization of all‐solid‐state sulfur cathodes reveals a significant disparity between material and electrode levels due to the high proportion of inactive components required for electro‐ionic transport. While the all‐electrochem‐active (AEA) electrode concept seeks to bridge this gap, fully realizing the energy‐density potential of sulfur‐based cathodes remains challenging. Here, we report a new strategy for co‐modulating the redox of the transition‐metal cation/sulfur anion to unlock the potential of the sulfur‐based electrode. By carefully adjusting the coordination between S anions and Ti cations, we constructed the AEA electrode with S‐anion (TiS x , x > 2)/Ti‐cation (amorphous TiS 2 ) co‐redox, where TiS x activates the redox activity of sulfur‐rich phases with narrower bandgaps through the reversible cleavage and recombination of S–S bonds, thereby enhancing the capacity utilization of anion‐redox in the electrode level, and amorphous TiS 2 serves as an electrochemically active matrix facilitating mixed ionic‐electronic conduction. This design eliminates inactive components and enables synergistic anion‐cation redox chemistry. Consequently, this designed cathode achieves an unprecedented electrode‐level energy density of 1829 Wh/kg, sustains an areal capacity of 11.6 mAh/cm 2 , and exhibits long‐term stability over 10 000 h. Device‐level demonstrations validate this synergistic approach as an effective design principle for realizing high‐energy‐density, long‐life all‐solid‐state battery cathodes under practical conditions.

Ionic liquids (ILs), renowned for their exceptional safety features, have become promising candidates for developing next-generation electrolyte systems in high-safety, high-energy-density lithium metal batteries (LMBs). However, the ability to precisely control the electric double layer (EDL) structure at the interface of IL-based electrolytes, based on ion geometry and short-range interactions, remains theoretically limited, which severely restricts the efficient and targeted selection of optimal IL structures. Guided by the Kornyshev model, this work demonstrates that IL electrolytes with smaller organic cations exhibit a higher packing parameter in the EDL, leading to denser ion packing and increased interfacial charge density. This ion-enriched EDL structure shows enhanced differential capacitance and significantly elevates the interfacial concentration of both Li+ and FSI- species. As a result, it enables rapid replenishment of Li+ ions during deposition and promotes the formation of a stable, anion-derived solid electrolyte interphase (SEI). Based on this mechanism, we designed a novel fluoropropyl pyrrolidinium-based IL electrolyte. The assembled LMBs using this electrolyte achieved a capacity of 4.5 Ah and an energy density of 505 Wh kg-1, exhibiting stable cycling performance and passing a rigorous nail penetration safety test. This study establishes a crucial link between the microscopic structure of the IL electrolyte-mediated electrified interface and macroscopic battery performance, offering new insights and direction for designing electrolytes for next-generation high-safety LMBs.

High-capacity Li-rich oxides are promising next-generation cathode materials for high-energy-density lithium-ion batteries. Significant efforts have been devoted to developing high-performance Li-rich cathodes, including both layered (LLRO) and disordered rock-salt (DRX) variants. However, their multiscale structural complexity, particularly associated with anionic redox reactions (ARR), has hindered a comprehensive understanding of the underlying mechanisms. Addressing these challenges requires advanced spectroscopic and structural characterization techniques that are sensitive to light elements and local atomic environments. In this Feature Article, we present our recent work employing two cutting-edge methods, resonant inelastic X-ray scattering (RIXS) and neutron pair distribution function (nPDF) analysis, to elucidate the structure-property relationships governing redox behavior and lithium diffusion in LLRO and DRX cathodes. We specifically examine ARR from a structural perspective, encompassing spectroscopic identification, local oxygen coordination, distorted oxygen pairs and spatial distribution of redox-active species. Furthermore, by combining nPDF with reverse Monte Carlo (RMC) modeling, we reveal the Li diffusion mechanisms in DRX materials across multiple scales, from local hopping channels and short-range ordering to long-range percolation pathways. These insights provide a foundation for the rational design of high-capacity and structurally stable oxide cathodes, and underscore the essential role of advanced characterization techniques in accelerating future battery research.

Divalent europium-activated phosphors have been a remarkable family due to coordination field-closely dependent multicolor luminescence characteristics. However, achieving efficient ultra-broadband white emission has been a great challenge. Herein, we report a Eu-activated ultra-broadband Ba5P6O20 phosphor with a full width at half maximum of up to 209 nm, coming from the multiple-site occupancy of Eu2+. Unfortunately, the internal quantum efficiency (IQE) is as low as 23%. Subsequently, the substitutional solid solution of Gd3+ for Ba2+ effectively promotes the reduction Eu3+ to Eu2+ and improves the IQE to 88%. The interstitial solid solution of Mg2+ regulates the Eu2+ occupancy sites, resulting in an additional emission centered at 407 nm. Finally, simultaneously dissolving Gd3+ and Mg2+ ions into Ba5P6O20 further improves the IQE (up to 94%) of the ultra-broadband emission. The incorporation of the studied ultra-broadband emitting phosphor with 365 nm LED chips realizes a high color rendering index warm white light output. Additionally, benefiting from the interstitial solid solution of Mg2+, the resulting material demonstrates promising static/dynamic anti-counterfeiting performance. This work establishes a substitutional-interstitial synergistic solid solution engineering, offering valuable insights for highly efficient ultra-broadband emission and multicolor luminescence of europium.

As the core determinant of lithium-ion battery performance, electrode materials play a crucial role in defining the battery's capacity, cycling stability, and durability. During charging and discharging, electrode materials undergo complex ion intercalation and deintercalation processes, accompanied by defect formation and structural evolution. However, the microscopic mechanisms underlying processes such as cation disordering, lattice oxygen loss, and stage structure formation are still not fully understood. To address these challenges, we have developed the Electrode Dynamic Ion Intercalation/Deintercalation Simulator (EDIS), a software platform designed to simulate the dynamic processes of ion intercalation and deintercalation in electrode materials. Leveraging high-precision machine learning potentials, EDIS can efficiently model structural evolution and lithium-ion diffusion behavior under various states of charge and discharge, achieving accuracy approaching that of quantum mechanical methods in relevant chemical spaces. The software supports quantitative analysis of how variations in lithium-ion concentration and distribution affect lithium-ion transport properties, enables evaluation of the impact of structural defects, and allows for tracking of both structural evolution and transport characteristics during continuous cycling. EDIS is versatile and can be extended to sodium-ion batteries and related systems. By enabling in-depth analysis of these microscopic processes, EDIS provides a robust theoretical tool for mechanistic studies and the rational design of high-performance electrode materials for next-generation lithium-ion batteries.

All-solid-state lithium-sulfur batteries (ASSLSBs) suffer from severe polysulfide shuttling and inadequate solid-solid interfacial contact, which restrict their practical application. Enhancing interfacial ion transport and polysulfide confinement is therefore critical for achieving high energy density and enabling use in electric aviation. Herein, we develop a composite solid-state electrolyte (DHCSE@PIL) integrating a covalent organic framework (COF) to suppress polysulfide shuttling and a poly(ionic liquid) (PIL) phase to improve interfacial ion transport. In this design, & horbar;SO3H-rich COF functions as functionalized fillers within the Li6.25Al0.25La3Zr2O12 (LALZO)/poly(ethylene oxide) matrix, enabling selective trapping of polysulfides, while in situ polymerization of pyrrolidinium-based ionic liquids (Pyr(13)TFSI) forms PIL "poly-ionic bridges" reinforcing electrode-electrolyte contact. Moreover, pyrrolidinium cations optimize lithium-salt coordination, facilitating Li+ transport and promoting a stable solid electrolyte interphase. Consequently, DHCSE@PIL exhibits an ionic conductivity of 0.74 mS cm(-1) and a Li+ transference number of 0.65. Li symmetric cells deliver stable plating/stripping for over 8000 h at 3 mA cm(-2), and Li|DHCSE@PIL|S full cells with high sulfur loading achieve 600 stable cycles at 0.5C. Furthermore, an Ah-level pouch cell delivers an energy density of 482 Wh kg(-1). This synergistic electrolyte/interfacial strategy provides insights into solid-state electrolyte engineering for advanced ASSLSBs.

The precise control of sulfide solid electrolyte (SSE) particle size distribution is crucial for constructing efficient ion-conducting networks in composite cathodes of all-solid-state lithium metal batteries (ASSLBs). This work systematically investigates the effects of key particle size parameters (D10, D50, D90) of Li6PS5Cl SSE on battery performance through controlled mechanical grinding. In this study, the optimal SSE particle size composition enables exceptional electrochemical performance of ASSLB: a high reversible capacity of 202.2 mAh/g at 0.25C, superior rate capability (76% capacity retention of 5C/0.25C), and outstanding cyclability (81.5% and 80% capacity retention after 4000 cycles at 3C and 5C, respectively). Microstructural analysis indicates that the optimized SSE particle configuration, when 7.3 ≤ D50Cathode/D50SSE and 2.0 ≤ D90Cathode/D90SSE ≤ 3.5, forms a hierarchical ion-conducting network. In this configuration, the fine particles of SSE in the composite cathode can effectively fill the cathode gaps, while the medium-sized particles can provide rapid ion transport channels, resulting in excellent rate performance and reversible capacity. Larger electrolyte particles will lead to insufficient interfacial contact and "island-like" ion transport paths. Additionally, excessively lowering D90 will also result in reduced battery performance (3.5 ≤ D90C/D90SE). This study provides quantitative guiding principles for SSE particle engineering.

Abstract Thermal runaway (TR) remains the most critical safety challenge limiting the large-scale application of lithium-ion batteries. A comprehensive understanding of the internal chain reaction mechanisms and their correlation with external early-warning signals is urgently required. This study establishes a stepwise analytical framework from single component and binary/ternary mixtures to full cells to bridge the gap between material-level reaction mechanisms and cell-level signal features. TG-DSC-MS experiments on designed component combinations revealed the underlying reaction mechanisms. These mechanisms were correlated with the synchronous evolution of multidimensional signals, including temperature, expansion force, voltage, and the concentrations of five characteristic gases (H2, CO, CO2, HF, and VOCs), during cell-level overheating tests. Through this cross-scale correlation, a three-stage “initiation-acceleration-runaway” chain-reaction pathway is identified for the first time at material level and subsequently validated against cell-level signal evolution, clarifying the transition from internal chemistry to observable failure. Specifically, the initiation stage is driven by cathode/electrolyte interfacial reactions, while the acceleration stage is governed by EC ring-opening polymerization occurring in the presence of lithiated graphite, and the runaway stage is triggered by the uncontrolled oxidative reactions initiated by cathode oxygen release. The TR process is further divided into five consecutive stages with distinct critical signal thresholds. Based on this mechanism-signal correspondence, a four-level hierarchical early-warning strategy is established, enabling early detection up to 698 seconds before TR. This work offers a viable pathway for translating mechanistic insights into quantifiable warning indicators, thereby bridging the gap between mechanistic understanding and engineering application.

Sulfide solid-state electrolytes (SSEs) for all-solid-state lithium batteries (ASSLBs) have garnered significant attention due to their ultra-high ionic conductivity and favorable processing characteristics. However, their widespread adoption is severely hampered by poor compatibility with lithium metal and inadequate air stability. Herein, we develop a novel solid electrolyte, Ultra-efficient and stable Janus interface to construct high-performance sulfide-based ASSLBs (LPSC-NdO), which simultaneously achieves high ionic conductivity (8.75 mS cm-1) and outstanding electrochemical stability. This SSE demonstrates exceptional interfacial compatibility for a critical current density of 6.62mAcm-2 and stable lithium plating/stripping for over 2000 hours in symmetric cells. Full ASSLBs employing LiCoO2 (LCO) cathode exhibit remarkable cycling stability, with 95.4% capacity retention after 1000 cycles at 1C. Moreover, LPSC-NdO possesses excellent air stability, releasing only a minimal amount of H2S (0.67 cm3 g-1) upon exposure to moisture. This work presents a feasible co-doping strategy for sulfide SSEs, offering useful insights for developing SSEs that balance air stability and lithium metal interfacial compatibility toward practical-oriented development.

Chlorine-based halide solid-state electrolytes (SSEs) have emerged as promising candidates for all-solid-state lithium batteries (ASSLBs) due to their high ionic conductivities and oxidative stability. Among them, LaCl3-based SSEs feature a non-close-packed lattice that provides intrinsically wide one-dimensional transport channels; however, their practical application is often constrained by rigid crystalline transport pathways and grain boundary resistance. Inspired by dual-anion engineering, by substituting LiCl with Li2O in Li0.388Ta0.238La0.475Cl3, a series of LaCl3-based composite electrolytes, Li2xTa0.25La0.5Cl2.75Ox (0.15 ≤ x ≤ 0.2, LTLCO), were synthesized. Atomic and local structure analysis reveals that, although elements are uniformly distributed at the macroscopic level, distinct local structural variations exist. Oxygen preferentially coordinates with Ta to form distorted octahedral Ta-Cl-O polyhedra, while the LaCl3 framework maintains structural integrity as a rigid backbone. The optimized Li0.35Ta0.25La0.5Cl2.75O0.175 SSE achieves a high ionic conductivity of 2.05 mS cm-1 at 30 °C and exhibits superior mechanical deformability, effectively mitigating interfacial failure in ASSLBs. ASSLBs assembled with LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes demonstrate exceptional rate performance and long-term cycling stability with 83.4% capacity retention after 300 cycles.

High-entropy alloys (HEAs) have garnered significant research interest owing to their exceptional catalytic properties in the degradation of organic pollutants. In this study, we report the synthesis of homogeneous FeCoNiCuAl HEA powders through an integrated single-roller melt-spinning and ball-milling approach. Compared to conventional gas-atomized counterparts, the ball-milled HEA powders demonstrate significantly enhanced catalytic performance in a Fenton-like system toward tetracycline (TC) degradation across varied temperature ranges. Notably, the BM-280 catalyst, processed at 280 rpm, achieves an outstanding TC removal efficiency of 94.8% within 60 min under H2O2 activation. The enhanced activity is attributed to the in situ generation of nanoscale active sites and a nanoporous structure, which synergistically promote reaction kinetics and interfacial mass transfer. These findings offer a novel and practicable strategy for designing advanced HEA-based advanced catalytic materials toward sustainable environmental purification.

Ring-opening polymerization (ROP) is widely employed for the in situ construction of solid polymer electrolytes (SPEs) in batteries due to the absence of byproducts. However, the thermal stability of such SPEs has long been overlooked. Here, we systematically investigate the thermal stability of two types of the most popular in situ ROP-prepared SPEs, including ether-based poly(1,3-dioxolane) (PDOL) and poly(1,3,5-trioxane) (PTXE), as well as ester-based poly(valerolactone) (PVL) and poly(trimethylene carbonate) (PTMC). Given the essential role of Li-salts in SPEs and the impossibility of removing ROP catalysts during in situ polymerization in cells, the thermal stability of ROP-prepared SPEs was evaluated in the presence of both components. The in situ ROP-prepared PDOL- and PTXE-based SPEs undergo rapid degradation into gases at 100 °C. The ROP and pyrolysis of PDOL/PTXE are demonstrated to share the same chemical mechanism and coexist in a temperature-dependent equilibrium, in which ROP is dominant at room temperature, while pyrolysis prevails at elevated temperatures and produces gases. The decomposition temperature of in situ ROP-prepared PVL and PTMC is around 180 °C, which is, however, decreased to 110 °C in the presence of Li-metal. This work reveals the challenges to the thermal stability of ROP-prepared SPEs and brings attention to the development of safer SPEs in solid-state batteries.

Hard carbon (HC) anode based solid-state sodium-ion batteries (SSIBs) possess highly intrinsic safety and cost effectiveness in the application of large-scale energy storage. However, it is hindered by large interfacial impedance and sluggish Na+ transport kinetics from the solid-solid electrode contact. Here, we propose an electrochemical presodiation strategy to in situ form a thin, uniform, and inorganic-rich (NaF/Na2O) solid-electrolyte interphase (SEI) on the HC anode. Such an SEI layer provides stable and good contact, leading to markedly reduced charge-transfer resistance and robust Na+ transport in a polymer-based solid electrolyte. The evidence for reversible Na+ insertion/extraction in the HC anode for SSIBs was first revealed by in situ X-ray diffraction. Consequently, the presodiated HC-based half-cell exhibits a reversible capacity of 275.2 mAh & centerdot;g-1 and good cycling stability with 90.9% retention after 100 cycles at 0.1 C. Finally, the presodiated HC-based SSIBs were constructed with the Na3V2(PO4)3 cathode, delivering a high capacity of 106.9 mAh & centerdot;g-1 at 0.1 C and good cycling stability without external pressure. These findings highlight inorganic engineering of the SEI as a powerful strategy for boosting interfacial kinetics toward regular pressure HC anode-based SSIBs.